The use of the organic As compound, roxarsone, as an antibiotic additive to poultry feed continues to raise concern over potential negative environmental impacts. Total As concentration in poultry litter can reach >40 mg kg−1 and both roxarsone and its mineralization product As(V) have been identified in poultry litters (PL). To investigate the fate of these As species upon land application of PL we conducted two studies. In the first, an Orangeburg soil (Ultisol from the Atlantic Coastal Plain) was spiked with either 20 mg kg−1 As(V) or roxarsone and incubated at 10% moisture content for 4 months. Exchangeable As was determined periodically by extraction with 0.1 M PO4. Both As(V) and roxarsone displayed similar desorption; initially, approximately 70% of added As was ligand exchangeable and this decreased to 35% after 4 months incubation, presumably due to either slow sorption reactions or a change in solid phase speciation of As to less exchangeable forms. In the second study, various manipulations of two PL samples were applied to the Orangeburg soil at realistic field application rates. The treatments were wet to 10% moisture content and water soluble As, Cu and organic carbon (DOC) was measured over 30 days. Arsenic and Cu solubility were highest from the dried litter samples. Ashing of the PLs decreased soluble As and Cu, presumably because of the loss of organic matter from the ashed litter and subsequent decrease in DOC. Application of leachates from either PL resulted in higher concentrations of soluble As and Cu than when the soil was amended with equivalent concentrations of soluble As and Cu dissolved in DI H2O. We hypothesize that the increased levels of DOC from the PL treatments enhance As and Cu solubility through competitive sorption and complexation, respectively. In fact, As and Cu solubility was correlated to DOC levels in the amended soil extracts. Even though land application of PL introduced relatively low concentrations of As and Cu to soil it appeared that other soluble constituents of PL significantly enhanced As and Cu solubility. 相似文献
The retention and fate of Roxarsone (ROX) onto typical reactive soil minerals were crucial for evaluating its potential environmental risk. However, the behavior and molecular-level reaction mechanism of ROX and its substituents with iron (hydr)oxides remains unclear. Herein, the binding behavior of ROX on ferrihydrite (Fh) was investigated through batch experiments and in-situ ATR-FTIR techniques. Our results demonstrated that Fh is an effective geo-sorbent for the retention of ROX. The pseudo-second-order kinetic and the Langmuir model successfully described the sorption process. The driving force for the binding of ROX on Fh was ascribed to the chemical adsorption, and the rate-limiting step is simultaneously dominated by intraparticle and film diffusion. Isotherms results revealed that the sorption of ROX onto Fh appeared in uniformly distributed monolayer adsorption sites. The two-dimensional correlation spectroscopy and XPS results implied that the nitro, hydroxyl, and arsenate moiety of ROX molecules have participated in binding ROX onto Fh, signifying that the predominated mechanisms were attributed to the hydrogen bonding and surface complexation. Our results can help to better understand the ROX-mineral interactions at the molecular level and lay the foundation for exploring the degradation, transformation, and remediation technologies of ROX and structural analog pollutants in the environment. 相似文献
Roxarsone (3-nitro-4-hydroxyphenylarsonic acid, ROX) has been widely used for decades as an organoarsenic feed additive to control intestinal parasites and improve feed efficiency in animal production. However, most of the ROX is excreted into the manure, causing arsenic contamination in wastewater. The arsenic compounds are toxic to microorganisms, but the influence of continuous ROX loading on upflow anaerobic sludge blanket (UASB) reactor is still unknown. In this study, the impact of ROX and its degradation products on the performance of the UASB reactor and the degradation and speciation of ROX in the reactor were investigated. The UASB reactor (hydraulic retention time: 1.75 d) was operated using synthetic wastewater supplemented with ROX for a period of 260 days. With continuous ROX addition at 25.0 mg·L–1, severe inhibition to methanogenic activity occurred after 87 days operation accompanied with an accumulation of volatile fatty acids (VFAs) and a decline in pH. The decrease of added ROX concentration to 13.2 mg·L–1 did not mediate the inhibition. As(III), As (V), MMA(V), DMA(V), HAPA and an unknown arsenic compound were detected in the reactor, and a possible biotransformation pathway of ROX was proposed. Mass balance analysis of arsenic indicated that 60%–70% of the arsenic was discharged into the effluent, and 30%–40% was precipitated in the reactor. The results from this study suggest that we need to pay attention to the stability in the UASB reactors treating organoarsenic-contaminated manure and wastewater, and the effluent and sludge from the reactor to avoid diffusion of arsenic contamination.